Enhanced photocatalytic NOx oxidation and storage under visible-light irradiation by anchoring Fe3O4 nanoparticles on mesoporous graphitic carbon nitride (mpg-C3N4)

[Display omitted] •Highly active and selective composite photocatalysts were developed for NOx abatement under visible-light illumination.•Structure of mesoporous graphitic (mpg) C3N4 was synthetically fine-tuned for optimum photocatalytic performance.•Photocatalytic NOx abatement activity, selectiv...

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Veröffentlicht in:Applied catalysis. B, Environmental Environmental, 2019-07, Vol.249, p.126-137
Hauptverfasser: Irfan, Muhammad, Sevim, Melike, Koçak, Yusuf, Balci, Merve, Metin, Önder, Ozensoy, Emrah
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Sprache:eng
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Zusammenfassung:[Display omitted] •Highly active and selective composite photocatalysts were developed for NOx abatement under visible-light illumination.•Structure of mesoporous graphitic (mpg) C3N4 was synthetically fine-tuned for optimum photocatalytic performance.•Photocatalytic NOx abatement activity, selectivity and reusability of C3N4 was further improved by Fe3O4-NP incorporation.•Fe2+/Fe3+ species increased oxygen reduction capacity of C3N4 resulting in lower NO2 production and higher selectivity.•Fe3O4/C3N4 photocatalyst had a positive DeNOx index, making it a viable DeNOx photocatalyst under VIS light at RT. Several mesoporous graphitic carbon nitride (mpg-C3N4) photocatalysts were synthesized by using a hard-templating method comprising thermal polycondensation of guanidine hydrochloride over silica spheres at three different temperatures (450, 500 and 550 ℃). After structural characterization of these mpg-C3N4 photocatalysts, they were tested in NO(g) photo-oxidation under visible (VIS) light. The effects of polycondensation temperature on the structure and photocatalytic performance of mpg-C3N4 in NO photo-oxidation were studied. The results revealed that polycondensation temperature has a dramatic effect on the photocatalytic activity of mpg-C3N4 in NO photo-oxidation, where mpg-C3N4 synthesized at 500 ℃ (mpg-CN500) showed the best performance in NOx abatement as well as a high selectivity towards solid state NOx storage under VIS light illumination. Photocatalytic performance of the mpg-CN500 was further enhanced by the anchoring of 8.0 ± 0.5 wt.% Fe3O4 nanoparticles (NPs) on it. Fe3O4/mpg-CN500 photocatalyst showed both high activity and high selectivity along with extended reusability without a need for a regeneration step. Enhanced photocatalytic NOx oxidation and storage efficiency of Fe3O4/mpg-CN500 photocatalyst was attributed to their mesoporous structure, high surface area and slow electron-hole recombination kinetics, efficient electron-hole separation and facile electron transfer from mpg-CN500 to Fe3O4 domains enhancing photocatalytic O2 reduction, while simultaneously suppressing nitrate photo-reduction and decomposition to NO2(g).
ISSN:0926-3373
1873-3883
DOI:10.1016/j.apcatb.2019.02.067